Miniaturized electrochemical sensors and their point-of-care applications

Most of the current analytical methods depend largely on laboratory-based analytical techniques that require expensive and bullky equipment,potentially incur costly testing,and involve lengthy detection processes.With increasing requirements for point-of-care testing(POCT),more attention has been paid to miniaturized analytical devices.Miniaturized electrochemical(MEC)sensors,including different material-based MEC sensors(such as DNA-,paper-,and screen electrode-based),have been in strong demand in analytical science due to their easy operation,portability,high sensitivity,as well as their short analysis time.They have been applied for the detection of trace amounts of target through measuring changes in electrochemical signal,such as current,voltage,potential,or impedance,due to the oxidation/reduction of chemical/biological molecules with the help of electrodes and electrochemical units.MEC sensors present great potential for the detection of targets including small organic molecules,metal ions,and biomolecules.In recent years,MEC sensors have been broadly applied to POCT in various fields,including health care,food safety,and environmental monitoring,owing to the excellent advantages of electrochemical(EC)technologies.This review summarized the state-of-the-art advancements on various types of MEC sensors and their applications in POCT.Furthermore,the future perspectives,opportunities,and challenges in this field are also discussed.     

Machine Learning towards Screening Solid-state Lithium Ion Conductors

Machine learning is an emerging method to discover new materials with specific characteristics.An unsupervised machine learning research is highlighted to discover new potential lithium ionic conductors by screening and clustering lithium compounds,providing inspirations for the development of solid-state electrolytes and practical batteries.     

Surface defect-rich ceria quantum dots anchored on sulfur-doped carbon nitride nanotubes with enhanced charge separation for solar hydrogen production

Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were synthesized via a thermal polycondensation coupled in situ depositionprecipitation method without use of template or surfactant.The structure and morphology studies indicate that ultrafine CeO2 QDs are well distributed inside and outside of SCN NTs offering highly dispersed active sites and a large contact interface between two components.This leads to the promoted formation of rich Ce³⁺ ion and oxygen vacancies as confirmed by XPS.The photocatalytic performance can be facilely modulated by the content of CeO2 QDs introduced in SCN matrix while bare CeO2 does not show activity of hydrogen production.The optimal catalyst with 10% of CeO2 loading yields a hydrogen evolution rate of 2923.8 μmol h-1 g-1 under visible light,remarkably higher than that of bare SCN and their physical mixtures.Further studies reveal that the abundant surface defects and the created 0 D/1 D junctions play a critical role in improving the separation and transfer of charge carriers,leading to superior solar hydrogen production and good stability.     

Superfast and solvent-free core-shell assembly of sulfur/carbon active particles by hail-inspired nanostorm technology for high-energy-density Li-S batteries

The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^-2 delivers a stable area capacity of 6.6 mAh cm^-2 over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^-2 over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.     

Unraveling the stabilization mechanism of solid electrolyte interface on ZnSe by rGO in sodium ion battery

Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.     

CXN天然沸石的研究2: 吸附性质

采用N~2,NH~3,CO~2,乙烯,丙烯,水,甲醇,乙醇,丙醇等作为吸附剂,研究了由我国CXN天然沸石改性制得的H-STI和Na-STI沸石的吸附性质,H-STI和Na-STI沸石的BET表面积及微孔孔体积约为420m^2/g和0.20m^3/g。根据NH~3和CO~2在H-STI沸石上的吸附等温线计算得到它们的吸附热分别为44.8和26.5kJ/mol。乙烯,丙烯,甲醇,乙醇,丙醇等在Na-STI沸石上的吸附等温线表明该沸石对有机分子的吸附具有链长选择性。在低分压下水相对于甲醇的吸附量表明沸石具有一定的疏水性质。     

常温常湿条件下Au/MeO~x催化剂上CO氧化性能

利用共沉淀法制备了Au/MeO~x催化剂(Me=Al,Co,Cr,Cu,Fe,Mn,Ni,Zn)。在常温常湿条件下,考察了不同氧化物负载的金基催化剂的CO氧化性能。结果表明,氧化物种类对催化剂的活性和稳定性均有较大的影响。Cu,Mn,Cr等氧化物负载的金基催化剂的活性较差,而Zn,Fe,Co,Ni,Al等金属氧化物负载的金基催化剂可将CO完全氧化,又具有一定的稳定性,在相同反应条件下,CO完全转化时的稳定性顺序为Au/ZnO>Au/α-Fe~2O~3>Au/Co~3O~4>Au/γ-Al~2O~3≈Au/NiO。还发现水对Au/MnO~x催化剂的活性和稳定性有负作用,而对180℃焙烧制备的Au/ZnO-180催化剂的活性和稳定性均有明显的湿度增强作用。     

Boost oxygen reduction reaction performance by tuning the active sites in Fe-N-P-C catalysts

Cost-effective atomically dispersed Fe-N-P-C complex catalysts are promising to catalyze the oxygen reduction reaction(ORR)and replace Pt catalysts in fuel cells and metal-air batteries.However,it remains a challenge to increase the number of atomically dispersed active sites on these catalysts.Here we report a highly efficient impregnation-pyrolysis method to prepare effective ORR electrocatalysts with large amount of atomically dispersed Fe active sites from biomass.Two types of active catalyst centers were identified,namely atomically dispersed Fe sites and Fe_xP particles.The ORR rate of the atomically dispersed Fe sites is three orders of magnitude higher than it of Fe_xP particles.A linear correlation between the amount of the atomically dispersed Fe and the ORR activity was obtained,revealing the major contribution of the atomically dispersed Fe to the ORR activity.The number of atomically dispersed Fe increases as the Fe loading increased and reaching the maximum at 1.86 wt%Fe,resulting in the maximum ORR rate.Optimized Fe-N-P-C complex catalyst was used as the cathode catalyst in a homemade Zn-air battery and good performance of an energy density of 771 Wh kgZn^-1,a power density of 92.9 m W cm^-2 at 137 m A cm^-2 and an excellent durability were exhibited.     

Regulation of carbon distribution to construct high-sulfur-content cathode in lithium-sulfur batteries

Lithium-sulfur(Li-S)battery is regarded as one of the most promising next-generation energy storage systems due to the ultra-high theoretical energy density of 2600 Wh kg^-1.To address the insulation nature of sulfur,nanocarbon composition is essential to afford acceptable cycling capacity but inevitably sacrifices the actual energy density under working conditions.Therefore,rational structural design of the carbon/sulfur composite cathode is of great significance to realize satisfactory electrochemical performances with limited carbon content.Herein,the cathode carbon distribution is rationally regulated to construct high-sulfur-content and high-performance Li-S batteries.Concretely,a double-layer carbon(DLC)cathode is prepared by fabricating a surface carbon layer on the carbon/sulfur composite.The surface carbon layer not only provides more electrochemically active surfaces,but also blocks the polysulfide shuttle.Consequently,the DLC configuration with an increased sulfur content by nearly 10 wt%renders an initial areal capacity of 3.40 mAh cm^-2 and capacity retention of 83.8%during 50 cycles,which is about two times than that of the low-sulfur-content cathode.The strategy of carbon distribution regulation affords an effective pathway to construct advanced high-sulfur-content cathodes for practical high-energy-density Li-S batteries.     

Confined Ni-In intermetallic alloy nanocatalyst with excellent coking resistance for methane dry reforming

Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming.Fortunately,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two major greenhouse gases into value-added syngas or hydrogen.The main problem retarding its industrialization is the seriously coking formation upon the nickel-based catalysts.Herein,a series of confined indium-nickel(In-Ni)intermetallic alloy nanocatalysts(In_xNi@SiO₂)have been prepared and displayed superior coking resistance for DRM reaction.The sample containing 0.5 wt.%of In loading(In_0.5Ni@SiO₂)shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability test.The boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of In.Both the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of methane.The reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood(L-H)mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS).This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases.     

Preparation of well-aligned carbon nanotubes/silicon nanowires core-sheath composite structure arrays in porous anodic aluminum oxide templates

The well-aligned carbon nanotubes (CNTs) arrays with opened ends were prepared in ordered pores of anodic aluminum oxide (AAO) template by the chemical vapor deposition (CVD) method. After then, silicon nanowires (SiNWs) were deposited in the hollow cavities of CNTs. By using this method, CNTs/SiNWs core-sheath composite structure arrays were synthesized successfully. Growing structures and physical properties of the CNTs/SiNWs composite structure arrays were analyzed and researched by the scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction spectrum (XRD), respectively. The field emission (FE) behavior of the CNTs/SiNWs composite structure arrays was studied based on Fowler-Nordheim tunneling mechanism and current-voltage (/-V) curve. And the photoluminescence (PL) was also characterized. Significantly, the CNTs/SiNWs core-sheath composite structure nanowire fabricated by AAO template method is characteristic of a metal/semiconductor (M/S) behavior and can be     

AAO模板法生长碳纳米管阵列及形成机理研究

采用阳极刻蚀法制备得到多孔氧化铝模板(AAO)，通过在二茂铁苯溶液中浸润而后热解的方法，得到内壁附着纳米铁颗粒的AAO模板。用化学气相沉积(CVD)法在AAO模板孔内生长出两端开口的碳纳米管(CNTs)阵列。仅用盐酸浸泡就可除去CNTs表面上的催化剂颗粒，得到高纯的CNTs阵列。高分辨透射电镜(HRTEM)和拉曼图谱(Raman)表明CNTs具有很低的石墨化结构。通过对CNTs形貌和形成过程的剖析，认为AAO模板孔道的导向作用以及模板孔内壁催化剂铁颗粒大小分布不均是形成低石墨化碳纳米管的主要原因。     

Application of Thermogravimetry and Differential Thermal Analysis in Catalytic CVD Synthesis of Carbon Nanotubes

Multi-walled carbon nanotubes (MW-CNTs) were prepared by chemical vapor deposition (CVD) method with the decomposition of acetylene over Co/SiO2 catalyst. TG-DTA technique was used together with TEM and XRD to study the effect of reaction temperature on the composition, graphitized extent, and diameter distribution of the produced raw CNTs based on their oxidization resistance. During the decomposition, the micro-crystallite of the active constituent (Co/SiO2) were growing up as the reaction temperature rising. This in turn resulted in an increase of the diameter distribution range of produced MW-CNTs. The average diameter increased from 20~30 nm (650℃) to 30~50 nm (750℃). XRD results also showed the graphitized extent of MW-CNTs was enhanced meanwhile the spacing between the layers (d002) decreased from 3.45 (650℃) to 3.32 (850℃) with the reaction temperature raised. TG-DTA data showed that the exothermic peak of the amorphous carbon was below 380℃and its content would decrease as temperature increasing. In summary, for CVD production of CNTs using acetylene gas on Co/SiO2 catalyst, low temperature (about 650℃) favored producing thinner MW-CNTs with the diameter from 20 to 30 nm while higher temperature (about 850℃) is favored thicker MW-CNTs (diameter from 70 to 100 nm).     

不同形貌碳纳米管的制备及其嵌锂性能研究

以乙炔作为反应气 ,用化学气相沉积法 (CVD)和模板法在不同温度 (60 0℃、70 0℃ )下制备了不同形貌的碳纳米管 ,并采用TEM ,HRTEM ,SEM ,XRD ,Raman和充放电实验方法研究其形貌、结构和电化学嵌锂性能 .结果表明 ,不同的制备方法及反应温度对碳纳米管的形貌、结构特征和电化学嵌锂性能均有明显的影响 .在制备的样品中 ,制备温度越低 ,样品的石墨化程度越差 ,可逆嵌锂容量相应越高     

ZnO纳米线阵列的电沉积法制备及表征(英文)

利用直流电沉积方法在多孔氧化铝模板的孔洞中生成锌纳米线,在氧气氛围中,于800°C下氧化2h,将氧化铝中的锌氧化成氧化锌.本研究利用氧气氛围进行锌的氧化,大大提高了传统方法的氧化锌纳米线的制备效率.用场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)和X射线衍射仪(XRD)对其形貌及成分进行表征和分析,结果表明,氧化铝模板的有序孔洞中填充了大尺寸、均匀连续的多晶态氧化锌纳米线.纳米线具有约1000:1的高纵横比,其长度等于氧化铝模板的厚度,直径约为80nm.光致发光(PL)光谱表明,氧化锌纳米线在504nm处有由于氧空位引起的较强蓝绿光发射.这为进一步研究ZnO/AAO组装体发学性质和开发新型功能器件提供了基础.     

Synthesis and modification of multi-walled carbon nano-tubes (MWCNTs) for water treatment applications

Synthesis of MWCNTs by chemical vapor deposition (CVD) of acetylene is investigated at different temperatures. Fe-Co/CaCO₃ catalyst/support prepared by wet impregnation method is used. CaCO₃ was found to be a good support as a high selective material for deposition of CNTs with high purity. The effect of temperature on catalyst/support phases and crystal size was identified by using XRD. The crystallite size was decreased with increase temperature. The effect of growing time and temperature on carbon yield was studied and the deposited MWCNTs increased with temperature. The structure and purity of synthesized CNTs at different temperatures was examined by TEM and the effect of temperature on the surface area of the synthesized MWCNTs was investigated, the surface area decreased as the temperature increased. The prepared CNTs were purified using chemical oxidation method and the effect of acid treatment on CNTs surface was examined by TEM and SEM. The function groups produced at CNTs surface were investigated by using FTIR spectroscopy also the effect of CNTs preparation temperature on FTIR spectra was studied. The functionalized CNTs were used for adsorption of some heavy metals and for removal of some organic dyes from water.     

微波等离子体辅助化学气相沉积法低温合成定向碳纳米管阵列

自碳纳米管被发现以来[1] ,这种准一维纳米新材料由于其优异的力学、电学、储氢等理化性质而显示出非常重要的理论研究与实际应用价值[2 ,3] .碳纳米管阵列更可作为场致发射器件 ,有望应用于冷阴极平板显示器或纳米电子学等前沿领域[4 ] ,成为碳纳米管研究中的热点 .在已有报道的多种制备碳纳米管阵列的方法中 ,以孔性硅或孔性 Al2 O3作为模板剂 ,通过化学气相沉积制备的方法较为普遍[5～ 7] ,但此类方法往往需要在较高温度 (高于 70 0℃[6 ,7] )下进行 ,对于碳纳米管阵列最诱人的应用前景之一平板显示器而言 ,要求在显示玻璃表面直接生长…     

CVD Growth of Carbon Nanotubes and Nanofibers: Big Length and Constant Diameter

Summary: We report mass production of carbon nanotubes (CNTs) and carbon nanofibers (CNFs) with relatively high length and aspect ratio. We synthesized carbon nanomaterials by chemical vapor deposition (CVD) of methane as the feeding gas on Fe/Mo nanoparticles that use alumina-aerogel support. Alumina-aerogel-supported Fe/Mo catalyst was prepared using sol-gel. Drying step performed using rotary evaporation and freeze-drying. CVD was performed using a quartz tube furnace. Samples were analyzed using scanning electron microscopy (SEM), Transmission electron microscopy (TEM) and Raman spectroscopy.     

Low‐Temperature Growth of Carbon Nanotubes Catalyzed by Sodium‐Based Ingredients

Synthesis of low‐dimensional carbon nanomaterials such as carbon nanotubes (CNTs) is a key driver for achieving advances in energy storage, computing, and multifunctional composites, among other applications. Here, we report high‐yield thermal chemical vapor deposition (CVD) synthesis of CNTs catalyzed by reagent‐grade common sodium‐containing compounds, including NaCl, NaHCO₃, Na₂CO₃, and NaOH, found in table salt, baking soda, and detergents, respectively. Coupled with an oxidative dehydrogenation reaction to crack acetylene at reduced temperatures, Na‐based nanoparticles have been observed to catalyze CNT growth at temperatures below 400 °C. Ex situ and in situ transmission electron microscopy (TEM) reveal unique CNT morphologies and growth characteristics, including a vaporizing Na catalyst phenomenon that we leverage to create CNTs without residual catalyst particles for applications that require metal‐free CNTs. Na is shown to synthesize CNTs on numerous substrates, and as the first alkali group metal catalyst demonstrated for CNT growth, holds great promise for expanding the understanding of nanocarbon synthesis.     

一种新的WO3纳米管的制备方法

一维纳米材料因可用来构造高性能纳米器件的结构单元而成为纳米材料研究的热点．目前的研究重点集中在材料的制备和结构性能表征方面,已发展了多种制备方法,主要有模板法、V-L-S法、L-L-S法和V-S法等,其中阳极氧化铝(AAO)模板法是制备一维材料的好方法．AAO模板的制备工艺已相当成熟,